LEI Li-jun , FAN Wei , HOU Feng-xiao , WANG Yue-qing , SUN Chuan , ZHANG Yi
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引用次数: 0
Abstract
The oxidation of alcohols is a significant chemical reaction, and the efficient oxidation of alcohols over heterogeneous catalysts using oxygen as oxidant has attracted much attention in recent years. Among them, Pd/CeO2 exhibits excellent alcohol oxidation performance. However, the structure-activity relationship between the catalyst's structure and its catalytic performance for alcohol oxidation is still not clearly understood. This study involved the preparation of CeO2 nanosheets with different concentrations of surface oxygen vacancies (Ov) and their subsequent loading with Pd to explore their catalytic performance for alcohol oxidation. The findings obtained through XPS, Raman, and XAS indicated a positive correlation between the surface Ov concentration of CeO2 as well as the ratio of Pd2+ fraction. The alcohol oxidation results and structure-performance relationship studies showed that there was a good linear relationship between the Pd2+ ratio as well as the surface Ce3+ concentration and the TOF of benzyl alcohol oxidation reaction, respectively. And the interfacial site (Pd–O–Ce) formed by Pd and CeO2 was the main catalytic site for this type of alcohol oxidation catalysts. This study contributes to the understanding of the catalytic role of interfacial sites in metal and oxide support for the development of better alcohol oxidation catalysts.
摘要醇的氧化是一种重要的化学反应,以氧为氧化剂在多相催化剂上高效氧化醇是近年来研究的热点。其中,Pd/CeO2表现出优异的醇氧化性能。然而,催化剂的结构与醇氧化催化性能之间的构效关系尚不清楚。本研究包括制备具有不同浓度表面氧空位(Ov)的CeO2纳米片,并随后负载Pd以探索其对酒精氧化的催化性能。通过XPS、拉曼和XAS分析发现CeO2的表面Ov浓度与Pd2+分数的比值呈正相关。醇氧化结果和结构性能关系研究表明,苯甲醇氧化反应中Pd2+比和表面Ce3+浓度与TOF分别呈良好的线性关系。Pd和CeO2形成的界面位点(Pd - o - ce)是这类醇氧化催化剂的主要催化位点。本研究有助于了解金属和氧化物载体中界面位点的催化作用,从而开发出更好的醇氧化催化剂。
期刊介绍:
Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.